Journal of Environmental Chemical Engineering ( IF 7.4 ) Pub Date : 2021-01-08 , DOI: 10.1016/j.jece.2021.105049 Yuhang Wang , Yunyun Xie , Changsen Zhang , Wenjun Chen , Jie Wang , Ruiqin Zhang , Haijian Yang
The oxygen mobility of BixCe1-x (x = 0, 0.1, 0.2, 0.3, 1) has been experimentally and theoretically investigated. The catalysts were synthesized by a simple co-precipitation method and used for soot combustion. As shown in Raman results, Bi0.2Ce0.8 has the largest amount of oxygen vacancies. The interaction of the Bi-Ce system is also presented in the outcomes of XPS, H2-TPR and O2-TPD, as well as the increased active oxygen species caused by the weakening of the metal-oxygen bond resulting from the oxygen mobility. Additionally, the electronic transfer between the Bi and Ce and the elongation of the Ce-O reported in the DFT studies support the synergism of Bi-Ce and the tuned mobility of oxygen. Further, the decrease of formation energy of oxygen vacancies presented in Bi0.2Ce0.8 in agreement with the experimental results. Moreover, the optimal adsorption capacity demonstrates excellent activity. Finally, we have well verified our previous proof that Bi0.2Ce0.8, which has a higher oxygen ion mobility, has the best catalytic performance under tight and loose conditions. Our work deepens the understanding of oxygen mobility over Bi-doped CeO2 and provides a strategy to promote the catalytic activity by tuning the oxygen mobility.
中文翻译:
通过双掺杂调节CeO 2的氧迁移率以用于柴油机烟尘氧化:实验和DFT研究
Bi x Ce 1-x(x = 0、0.1、0.2、0.3、1)的氧迁移率已通过实验和理论研究。该催化剂通过简单的共沉淀法合成并用于烟灰燃烧。如拉曼结果所示,Bi 0.2 Ce 0.8具有最大的氧空位。XPS,H 2 -TPR和O 2的结果也显示了Bi-Ce系统的相互作用。-TPD,以及由氧迁移率引起的金属-氧键减弱导致的活性氧种类增加。此外,DFT研究中报道的Bi与Ce之间的电子转移以及Ce-O的延伸支持了Bi-Ce的协同作用和调节的氧迁移率。此外,Bi 0.2 Ce 0.8中氧空位形成能的降低与实验结果一致。而且,最佳的吸附容量显示出优异的活性。最后,我们已经很好地验证了我们先前的证明Bi 0.2 Ce 0.8具有较高的氧离子迁移率,在严密和宽松的条件下具有最佳的催化性能。我们的工作加深了对Bi掺杂CeO 2上氧迁移率的理解,并提供了一种通过调节氧迁移率来提高催化活性的策略。